Cylindrical protein nanotubes comprising a layer-by-layer (LbL) assembly of human serum albumin (HSA) with polycations [polyallylamine hydrochloride (PAH), poly-L-arginine hydrochloride (PLA), and poly-L-lysine hydrobromide (PLL)] have been prepared using template synthesis with a porous anodic aluminum oxide (AAO) membrane. Visible absorption spectra of the multilayered thin film of the polycation and HSA on a quartz plate showed alternate LBL film formation of (polycation/HSA)(n).