Nanocellulose has gained increasing interest due to its excellent properties and great potential as a functional component or carrier in food and pharmaceutical industries. This study investigated the structural, thermal, and physicochemical properties of nanofibrillated cellulose (NFC) and nanocrystalline cellulose (CNC) extracted from bamboo shoot (Leleba oldhami Nakal) processing byproducts. NFCs were prepared through low concentration acid hydrolysis combined with ultrasonic treatment. CNCs were further isolated from NFCs using sulfuric acid hydrolysis treatment. TEM images showed that NFC and CNC exhibited typical long-chain and needle-like structures, respectively. CNC suspension was stable due to its zeta potential of -34.3 ± 1.23 mV. As expected, both NFC and CNC displayed high crystallinity indexes of 68.51 and 78.87%, and FTIR analysis confirmed the successful removal of lignin and hemicellulose during the treatments. However, the thermogravimetric analysis indicated that sulfuric acid hydrolysis decreased the thermal stability of CNCs. The improved physicochemical properties of NFC and CNC suggested their potential in various applications.