Starring screen roles in the 1950s soon evaporated, and Herbert was relegated to TV appearances in the 1960s. Growing into that typically awkward teen period, he was forced to subsist on whatever episodic roles he could muster, including bits on Wagon Train (1957), Rawhide (1959), The Twilight Zone (1962), The Fugitive (1963), Hazel (1963), Family Affair (1966), and My Three Sons (1966).

Blue eyed and freckle-faced, Herbert began his acting career at age four when he appeared on the television series Half Pint Panel (1952). The Long, Long Trailer (1954) would have been his first movie, just after he appeared in the stage production of On Borrowed Time at the Rancho Theatre. However, after auditioning with some 40 other kids and chosen for a role, he was cut from the film.

What followed included roles in such popular and cult films as The View from Pompey's Head (1955); The Night Holds Terror (1956); These Wilder Years (1956), with James Cagney and Barbara Stanwyck; Gunfight at the O.K. Corral (1957); The Colossus of New York (1958); The Fly (1958); Houseboat (1958); The Man in the Net (1959), with Alan Ladd; The Five Pennies; Please Don't Eat the Daisies (1960); and 13 Ghosts (1960), in which producer/director william Castle gave him top billing at the age of 12 in order to secure his services.

This period was highlighted by a celebrated performance at age eight for his role as a blind child on an episode of Science Fiction Theater (1956). Airing December 22, 1956, "The Miracle Hour" episode is about a man who never gives up hope that his fiancée's blind six-year-old son will not have to spend the holidays in darkness. Herbert starred with Dick Foran and Jean Byron. Five years later he played the son of a blind man (Rod Steiger) in an episode of NBC's Wagon Train

He expressed deep appreciation of the work Paul Petersen's organization, A Minor Consideration, does by assisting present and former child actors both financially and emotionally. Herbert and Petersen played brothers together in the film Houseboat (1958), starring Cary Grant and Sophia Loren, and he guest-starred four times as David Barker from 1958 to 1960 on Petersen's ABC series, The Donna Reed Show.

During his peak, he was performing nonstop with multiple projects completed each year. By 1959, Herbert had achieved a lofty place among the most-desired and highest-paid child actors of his time, making nearly $1,650 per week. He had established for himself both the reputation and the nickname of "One-Take Charlie." Of his acting style, one reviewer described Herbert as "sincere, accurate, overenunciated at times, like a storybook character come to life. An extraordinary child actor by any standard. Herbert’s intense emotive quality is very much of the method acting school, highly unusual in such a young performer."

With no family of his own, it took Herbert nearly forty years to turn his life around. Clean and sober since August 2004, his films—now reaching new generations of fans via DVD and cable TV—and his appearances at science fiction film festivals and conventions sustained him.

Charles Herbert appeared annually for six years in the Celebrity lineup at the Monster Bash, held each June, at the Pittsburgh, Pennsylvania Airport Four Points with his The Boy and the Pirates costar Susan Gordon. He died in Las Vegas on October 31, 2015, from a heart attack.

Describing his studio education as "nonexistent," Herbert attended public schools (Melrose, Bancroft, Fairfax High) rather than one of the private schools tailored to the unique needs of child actors. "My parents made that mistake, without malice; they were not too familiar [with the problems that child actors face]." Herbert made up a story that he had a twin brother and that it was not him whom his classmates were seeing in movies and on TV. Referencing his role in the sci-fi movie classic The Fly, he said, "Back in those days, the very few people who did know I was an actor, when they were kidding me, they’d go, Help me, help me, help meeee!"...