Mature pods of Leucaena leucocephala (Lam.) de Wit were utilized as raw material for nanocrystalline cellulose (NCC) production. NCC’s isolation begins with L. leucocephala fiber’s alkaline treatment with sodium hydroxide, followed by bleaching treatment at three different percentages (3%, 5%, and 7%) of sodium hypochlorite. Acid hydrolysis was then conducted to obtain NCC, which was comprehensively characterized in terms of morphology, chemical functional groups, whiteness index, and crystallinity. Fourier-transform infrared spectroscopy (FTIR) and chemical composition results showed that alkali treatment (NaOH) and bleaching (3%, 5%, and 7% of sodium hypochlorite, NaClO) were effective in the removal of lignin and hemicellulose. The variation of sodium hypochlorite concentration affected physical and structural characteristics of the NCC produced, which exhibited a rod-shaped structure with diameters ranging from 17 to 49 nm. These observations provide insight into the potential utilization of L. leucocephala as raw material for preparing nanocellulose, which may address problems of the underutilized mature pods.