Bloom credits Tony Richardson, who guided her opposite Burton in the film version of "Look Back in Anger", with giving her "the courage to experiment", and she reunited with the director many years later for the 1988 CBS miniseries "Beryl Markham" A Shadow in the Sun". She also acted with Burton in "Alexander the Great" (1956) and "The Spy Who Came in from the Cold" (1965), saying in PEOPLE (October 28, 1996) that their relationship was "brilliant, unspoiled and pure" while admitting that "he went from a naive young boy from Wales to a rather practiced seducer." (Their romance finally ended when she caught him in the arms of Susan Strasberg.) Bloom has married only one actor, Rod Steiger (her co-star in Broadway's "Rashomon" 1959), with whom she starred in "Three Into Two Won't Go" and "The Illustrated Man" (both 1968). She also portrayed a young woman of decidedly unnatural instincts in Robert Wise's "The Haunting" (1963) and a sympathetic caseworker opposite Oscar-winner Cliff Robertson in "Charly" (1968), among her other films of the 60s.

Bloom made her American TV debut as Roxanne to Jose Ferrer's "Cyrano de Bergerac" for "Producer's Showcase" (NBC, 1955) and returned to that network in the title female roles of "Caesar and Cleopatra" (1956) and "Romeo and Juliet" (1957). Her small screen turns over the next 22 years were rare (e.g., Queen Anne in "Soldier in Love" 1967), but beginning with 1979 appearances in "Henry VIII" (PBS, as Queen Katherine) and "Backstairs at the White House" (NBC, as Edith Galt Wilson), she became a frequent TV presence. Particularly memorable in an Emmy-nominated turn as Lady Marchmain opposite Olivier in the acclaimed British miniseries "Brideshead Revisited" (PBS, 1982), she worked throughout the decade in quality projects like John Schlesinger's remake of "Separate Tables" (HBO, 1983), the "American Playhouse" (PBS) adaptation of third husband Philip Roth's "The Ghost Writer" (1984), the BBC's "Shadowlands" (1985, for which she won a BAFTA Award) and the highly-acclaimed ABC miniseries "Queenie" (1987), not to mention a return to the classics as Oedipus' wife-mother Jocasta in "Oedipus the King" ("The Theban Plays", PBS 1988).

After her fine supporting work in "Sammy and Rosie Get Laid" (1987), Bloom upped her profile considerably as the loyal wife of Martin Landau in Woody Allen's "Crimes and Misdemeanors" (1989) and later appeared in the chorus of Allen's "Mighty Aphrodite" (1995). Her best exposure of the 90s, however, came not as an actress but as the writer of a 1996 tell-all memoir, "Leaving a Doll's House", which focused primarily on the disintegration of her marriage to novelist Philip Roth. Though she had sunk her teeth into the prototypical feminist role of Nora in Henrik Ibsen's "A Doll's House" on several occasions during the 70s, the actress had been unable to overcome her own passivity within a male-dominated relationship, and the book registered her shock at being left by a man she both feared and loved after nearly 20 years together. Bloom made a rare TV appearance as the villainous Orlena Grimaldi on the CBS daytime drama "As the World Turns" in 1995 and appeared in features (i.e., "Daylight" 1996) and TV-movies ("What the Deaf Man Heard", CBS 1997), but her most powerful work at the end of the 20th Century came onstage as the vengeful matriarch Clytemnestra in David Leveaux's 1998 production of Sophocles' "Electra", which returned her to Broadway for the first time in 22 years and garnered her a Tony nomination.