With vivid interest in nature, Kjærbølling used here all his spare time to pursue botanical studies and observe bird life. 1843 he published a handbook of outdoor and flower gardening, and the following year, he gained the post of inspector at the Jutland, Funen and Schleswig created gardens at Snoghøj.
His more famous works include Ornithologia danica, Danmarks Fugle (Birds of Denmark or "national birds"), produced during 1847-1852, and his collection titled Skandinaviens Fugle (Birds of Scandinavia) which are descriptions of birds accompanied by lithographed drawings of the birds on hand-coloured plates. His works became very popular and spread public interest in Danish birds and bird spotting.
In 1832 he married Christine Ploug-Nissen (b. July 21, 1878).
In 1859 he founded the Copenhagen Zoo in "Prinsess Vilhelmines Have" (The garden of Princess Vilhelmine) at Frederiksberg Palace which was given to him by the chief directorate of Copenhagen as recognition for his work. After his death the garden was inherited by his son Frederick Hugo Kjærbølling (1844-1904), who in 1872 handed it over to a company.