© 2016 American Chemical Society. Rice straw cellulose was completely defibrillated via aqueous counter collision (ACC) at a low energy input of 15 kWh/kg, then fractionated by differential centrifugation into four increasing weight fractions of progressively thinner cellulose nanofibrils (CNFs): 6.9% in 80-200 nm, 14.4% in 20-80 nm, 20.3% in 5-20 nm, and 58.4% in less than 5 nm thickness. The 93.1% less than 80 nm or 78.7% less than 20 nm thick CNFs yields were more than double those from wood pulp by other mechanical means but at a lower energy input. The smallest (3.7 nm thick and 5.5 nm wide) CNFs were only a third or less in lateral dimensions than those obatined through ACC processed from wood pulp, bamboo, and microbial cellulose pellicle. The less than 20 nm thick CNFs could self-assemble into continuous submicron (136 nm) wide fibers by freezing and freeze-drying or semitransparent (13-42% optical transmittance) film by ultrafiltration and air-drying with excellent mechanical properties (164 MPa tensile strength, 4 GPa Young's modulus, and 16% strain at break). ACC defibrillated CNFs retained essentially the same chemical and crystalline structures and thermal stability as the original rice straw cellulose and therefore were much more thermally stable than TEMPO oxidized CNFs and sulfuric acid hydrolyzed cellulose nanocrystals from the same rice straw cellulose.