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This study investigates the physical, mechanical, and structural characteristics of handmade paper samples derived from cellulose extracted from grass clippings using two distinct methods as follows: (1) alkali treatment and (2) alkali treatment followed by bleaching, coupled with the incorporation of barium sulfate as a mineral filler. Our investigation revealed that the handmade paper samples’ densities, moisture contents, and thicknesses varied within the ranges of 0.436 to 0.549 g/cm3, 5.60 to 2.51%, and 0.41 to 0.50 mm, respectively. The tensile strength and folding endurance of the papers produced through alkali treatment with barium sulfate were notably superior to those produced from bleached pulp and barium sulfate. Our analysis indicates that several critical factors, including paper density, thickness, the crystallinity index, and the microfibrillar structure of cellulose, intricately influence the mechanical and strength properties of the samples. Using Fourier transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) techniques, we identified characteristic cellulose bonds and examined cellulose’s crystalline and amorphous phases. Additionally, the crystallinity index of the samples was determined using both the Segal and peak deconvolution methods. Scanning electron microscopy (SEM) micrographs revealed interconnected networks of cellulose fibers with varying thicknesses and lengths, along with incorporated mineral filler within the cellulose fiber structure. Variations in mineral particle retention were attributed to the presence or absence of cellulose microfibrils. These findings contribute to our understanding of the observed strength characteristics of the paper samples and underscore the potential applications of cellulose derived from grass clippings, especially when combined with barium sulfate as a mineral filler in paper production.