On leaving school Albery entered an architect"s office, and started to write plays. His farce A Pretty Piece of Chiselling was given its first production by the Ingoldsby Club in 1864. After some failures, his adaptation, Doctor Davy, was produced at the Lyceum Theatre, London (1866).
His most successful piece, Two Roses, a comedy, was produced at the Vaudeville Theatre in 1870, in which Sir Henry Irving made one of his earliest London successes as Digby Grant.
The production ran for 300 performances. He also wrote the farce Brighton (1888) among other later plays.
Albery also wrote a book called Where"s the Cat? in 1880. Albery"s and Moore"s son was Bronson Albery (1881-1971), a theatre director, after whom the Albery Theatre is named.
He wrote this epitaph for himself: "He slept beneath the moon/He basked beneath the sun;/He lived a life of going-to-do,/And died with nothing done.".