For the next several months Vivien worked on stage and appeared in two minor films; The Village Squire, a comedy, and Gentleman's Agreement, in which she played an unemployed typist. Her husband Leigh, felt this was just a fling with acting - one that would soon get out of her system. He hoped she would return to her domestic role of wife and mother, but it now seemed unlikely - Vivien was determined to continue acting.

In the spring of 1935, Vivien's talent agent succeeded in getting her a part in a comedy entitled Look Up and Laugh, starring Gracie Fields - George Burns wife and comedy partner. During this time, she auditioned for a leading role in a costume play called The Mask of Virtue. Her acting skills from her work at the academy had improved enough that Vivien succeeded in winning the part. After several months of rehearsals while continuing to work in the studio on her 4^th film, the The Mask of Virtue opened on May 15th, 1935. The play was a great success and Vivien became an overnight sensation. Alexander Korda, the famous European film producer, happened to be present on opening night (invited by the play's director) and he asked her to sign a contract that would guarantee 50 thousand pounds over a 5 year period. This contract, if it had been completed, would have resulted in 10 films in Britain from the period between 1935 and 1940. Vivien ended up making only 6 films before leaving for Hollywood in 1938.

After The Mask of Virtue ended its run, Vivien waited for another success to feed her new found fame, but it did not arrive as easily. The remainder of 1935 was slow, and she performed in a few more plays of less importance. One thing of note did occur however - she was introduced to her matinee idol, Laurence Olivier, at the trendy Savoy Grill in London.

Laurence Olivier was 7 years her elder, born in Dorking, England, of Anglo-Catholic parents. He obtained a scholarship to the Central School of Speech and Drama, and made his way to the London stage by the time he was 21. He married his first wife, Jill Esmond Moore, also an actress in July of 1930. When Olivier was 28, he went to Hollywood and made three minor films, returning to England in 1932, unhappy with the results. Soon after, he acquired success as a matinee stage idol, performing in various works including Shakespeare. In August 1936, he was asked to co-star in what would be Vivien's first film for Alexander Korda, Fire Over England. Olivier played a sailor sent to Spain on an important mission for the Queen. Vivien played Cynthia, the Queen's lady-in-waiting, and his new found love. This film gave the two rising stars time to spend with each other on screen and off, and their relationship grew stronger. It was long hours of work and they spent whatever chance they could together alone. Shooting Dark Journey started immediately afterward for Vivien, co-starring Conrad Veidt. She had the leading role in a spy drama about a clothing shop owner who worked secretly for the government.

To continue her new film contract, Vivien was then due to star in Storm in a Teacup, the first of two films working opposite Rex Harrison. She took a short break in Rome with Olivier before returning to the studio to begin shooting. During this period Vivien read a great deal during breaks on set and found a new favourite novel that she re-read several times - Gone With the Wind. She even asked her agent to submit her name to the widely publicized search to find an actress for Scarlett O'Hara.

This request was returned with a reply:

To continue her contract with Alexander Korda, Vivien would now star in a second feature alongside Olivier, entitled Twenty-One Days. A low budget drama about a convicted killer and the wife of the murdered man. Filming began in May of 1937, scripted by Graham Greene. On June 16^th, after a brief run on stage in Hamlet, again opposite Olivier, Vivien left her husband Leigh, moving to Chelsea with her new found love. Their secret affair had gone as far as it could, as did each of their marriages. On the set, the conversation turned to the topic of the day - the casting of Gone With The Wind:

Since Vivien was now living with Olivier, her daughter Suzanne was in the care of Gertrude, Vivien's mother. The next few years for the new couple would be spent waiting for an official divorce. Vivien was loaned to MGM to make A Yank at Oxford to increase her American exposure - a move that would benefit both Alexander Korda's role as her producer and Vivien's career, especially if she was to be considered for the role of Scarlett O'Hara. She worked on A Yank at Oxford during the autumn of 1937 with her former convent schoolmate, and now actress, Maureen O'Sullivan, while Olivier shot The Divorce of Lady X with Merle Oberon.

1937 had ended and a new year of work began. Vivien started shooting St. Martin's Lane in January 1938. This was her 9th film, and co-starred Charles Laughton and Rex Harrison. She played a busker that rises to stardom in London. When it was released, the reviews were positive, stating that Vivien had improved her acting enough to stand alongside Charles Laughton on screen. Laurence Olivier was just as busy. He was asked to play the part of Heathcliff opposite Merle Oberon in a Hollywood production of Wuthering Heights. Accepting this offer, he left England on November 5^th 1938 - Vivien's 25^th birthday. Wanting to be with him as soon as possible, she abandoned her winter plan of performing in A Midsummer Night's Dream at the Old Vic, and left heading towards California on Saturday November 27^th for a two week trip "…partly because Larry is there, and partly because I intend to get the part of Scarlett O'Hara". It was a journey that would not only change Vivien's career - but would change the search for Scarlett forever…