During this period, The Stage recorded, Laye "was dated by a handsome young actor called James Baumgarner, whose career took off when he changed his surname to Garner".
Although the stage remained her first love, Laye made several films in the 1950s. and Blue Murder at St Trinian's and Jasmine Hatchet in Doctor at Large in 1957.
One of the few failures of Laye's stage career came in 1957 with The Crystal Heart at the Saville Theatre, London. Ned Sherrin described the piece as "a disastrous camp American musical". The production closed after five performances. At Her Majesty's Theatre in December 1957 Laye played Estell Novick in a non-musical comedy, The Tunnel of Love. Despite mixed notices for the play, Laye and her co-star Carmichael were praised, and the piece ran for more than a year. Laye then joined Joan Littlewood's Theatre Workshop company to play Redhead in a musical adaptation of Wolf Mankowitz's novel Make Me an Offer, seen first at the Theatre Royal, Stratford East in October 1959 and then at the New from December. but she later commented that she did not work with Littlewood again, "and you can draw your own conclusions from that". On television she appeared in an episode of the BBC television sitcom The Rag Trade in 1962 and in 1965 she co-starred with her friend Sheila Hancock in six episodes of the sitcom The Bed-Sit Girl. After that she appeared in the West End comedy Say Who You Are with Carmichael, Cargill and Jan Holden. In 1967 she had a cameo role in Charlie Chaplin's romantic film comedy A Countess from Hong Kong, playing a scene opposite Marlon Brando. The following year she toured as Miriam in Gwyn Thomas's comedy, The Keep. The following year she made her first appearance with the Royal Shakespeare Company (RSC), playing Theresa Diego in Barnes's historical drama The Bewitched. She continued in the role in May 1974 when the production transferred to the Aldwych Theatre, London. Two years later, at the Old Vic, Barnes directed The Frontiers of Farce, a double bill of his adaptations of one-act plays by Frank Wedekind and Georges Feydeau, in which Laye starred with Leonard Rossiter, John Stride and John Phillips. Actress and playwright worked together on three more radio presentations in the 1970s: his adaptations of Wedekind's Lulu, in which she played Countess Geschwitz (1978) and of Thomas Middleton's A Chaste Maid in Cheapside, described in the Radio Times as "a bawdy Jacobean black comedy", She had leading roles in two further Barnes adaptations for the BBC: Helen in Wedekind's The Singer and Catherine in Feydeau's Le Bourgeon, given as The Primrose Path (1984). and Ruth in a version of The Pirates of Penzance at the Manchester Opera House with Michael Ball as Frederic and Paul Nicholas as the Pirate King in 1985. Laye's later RSC appearances were as Maria in Twelfth Night (1996) and Mrs Medlock in the musical The Secret Garden (2000 and 2001). Her later West End credits included the musicals Nine in 1997 and Into the Woods in 1998, both at the Donmar Warehouse, a Mother Courage figure in Barnes's mediaeval play Dreaming at the Queen's (1999), Elizabeth II in Single Spies in 2000, and Mrs Pearce in Trevor Nunn's revival of My Fair Lady at the Theatre Royal, Drury Lane in 2002.
Laye featured as Madame de Rosemond in a revival of Christopher Hampton's Les Liaisons Dangereuses at the Playhouse Theatre in 2004, receiving the Clarence Derwent Award for best supporting actress. In 2005, she toured Britain as the Grandmother in Roald Dahl's The Witches. Her later television work included Mrs Sparsit in Barnes's adaptation of Hard Times, and character roles in EastEnders, Coronation Street, Holby City, Midsomer Murders, Doctors, The Amazing Mrs Pritchard, and The Commander.