Novel [Cr-III(amp)(bipy)(Cl)] (1) (H(2)amp = N-(hydroxyphenyl)salicyldimine; bipy = 2,2'-bipyridyl) and [Cr-III(app)(bipy)(Cl)](+) (2) (H(2)app = N-(hydroxyphenyl)pyridine-2-carboxaldimine bipy = 2,2'-bipyridyl) complexes have been synthesized and characterized by physico-chemical methods. Complexes 1 and 2 have been employed as catalysts in the oxidation of both saturated and unsaturated hydrocarbons using tert-butylhydroperoxide (t-BuOOH). The significance of the results with respect to oxo-functionalization of C-H bonds both in unsaturated and saturated hydrocarbons is noted.