Synthesis of copper sulfide and stable copper (Cu(0)) nanoparticles in Langmuir-Blodgett films of the amphiphilic benzilidine derivative 2,4-dihydroxybenzilidine-4＇-(hexadecylamino)benzylamine (BHDB) has been investigated using (i) sulfidation (S) by treating copper complex of BHDB in Langmuir-Blodgett film (LB film) with sodium sulfide and (ii) hydrogenation (H) using hydrogen gas. X-ray photoelectron spectroscopy, UV-visible absorption spectroscopy, and optical microscopy indicated the formation of nanocrystallites of copper ranging in size from 4 to 10 nm.