ABSTRACTCellulose nanocrystals have emerged as replacements for man-made fibers to fabricate environmentally friendly green products. In this work, cellulose nanocrystals (CNCs) of mixed morphology were synthesized by acid hydrolysis of compost using sulfuric acid. Compost, an agro-based biomass feedstock, procured from water hyacinth (Eichhornia crassipes), cow dung, and saw dust (8:1:1) was utilized for the extraction of cellulose, followed by synthesis of CNCs. Compost was prepared using a rotary drum composter and was utilized for the production of CNCs. A two-step procedure for the extraction of CNCs was studied. Initial chemical treatments, including alkali treatment and bleaching, led to the gradual removal of lignin and hemicellulose, while the subsequent sulphuric acid (40%) hydrolysis step yields CNCs in an aqueous suspension. The synthesized CNCs have been studied by Fourier transform infrared (FTIR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and particle size analyzer. The morphology and dimension of nanofibrils were studied by scanning electron microscopy (SEM), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and atomic force microscopy (AFM) techniques, which showed mixed morphology of rectangular cone type and spherical dimensions. Fabrication of such mixed morphology was found to be dependent on the selected biomass. The trace of metal elements present in the biomass was investigated by scanning electron microscopy-energy dispersive X-ray (SEM-EDX). We report a cost effective and feasible approach of utilizing inexpensive bioresources for production of value added products like CNCs, which could find potential application in the fields of healthcare, biomedical engineering, packaging, etc.