Regenerated cellulose nanoparticles (RCNs) including both elongated fiber and spherical structures were prepared from microcrystalline cellulose (MCC) and cotton using 1-butyl-3-methylimidazolium chloride followed by high-pressure homogenization. The crystalline structure of RCNs was cellulose II in contrast to the cellulose I form of the starting materials. Also, the RCNs have decreased crystallinity and crystallite size. The elongated RCNs produced from cotton and MCC had average lengths of 123 ± 34 and 112 ± 42 nm, and mean widths of 12 ± 5 and 12 ± 3 nm, respectively. The average diameter of spherical RCNs from MCC was 118 ± 32nm. The dimensions of the various RCNs were all well fitted with an asymmetrical log-normal distribution function. The RCN has a two-step pyrolysis, different from raw MCC and cotton that have a one-step process.