Cellulose nanoparticles (CNPs) were prepared from microcrystalline cellulose using two concentration levels of sulfuric acid (i.e., 48 wt% and 64 wt% with produced CNPs designated as CNPs-48 and CNPs-64, respectively) followed by high-pressure homogenization. CNP-reinforced polymethylmethacrylate (PMMA) composite films at various CNP loadings were made using solvent exchange and solution casting methods. The ultraviolet-visible (UV-vis) transmittance spectra between 400 and 800 nm showed that CNPs-64/PMMA composites had a significantly higher optical transmittance than that of CNPs-48/PMMA. Their transmittance decreased with increased CNP loadings. The addition of CNPs to the PMMA matrix reduced composite’s coefficient of thermal expansion (CTE), and CNPs-64/PMMA had a lower CTE than CNPs-48/PMMA at the same CNP level. Reinforcement effect was achieved with the addition of CNPs to the PMMA matrix, especially at higher temperature levels. CNPs-64/PMMA exhibited a higher storage modulus compared with CNPs-48/PMMA material. All CNP-reinforced composites showed higher Young’s modulus and tensile strengths than pure PMMA. The effect increased with increased CNP loadings in the PMMA matrix for both CNPs-64/PMMA and CNPs-48/PMMA composites. CNPs affected the Young’s modulus more than they affected the tensile strength.