Sugarcane rind fiber/natural latex biodegradable composites were prepared by compounding natural latex with sugarcane rind fiber as reinforcing filler. We selected three chemical solvents, including sodium hydroxide (NaOH), silane (KH550) and acrylic acid (AA), and used one-step or two-step treatment method to improve the interfacial adhesion between sugarcane rind fiber and natural latex matrix. Fourier Transform Infrared spectroscopy (FTIR) was used to characterize the chemical composition change at the sugarcane rind fiber surface structure by the chemical treatments. Scanning Electron Microscopy (SEM) results showed that the interfacial adhesion and dispersion of the composites based on two-step treated fiber were improved. The mechanical properties of these biodegradable composites were evaluated, which showed an increase of the tensile strength and elongation at break of the composites based on two-step treated fiber compared to those based on untreated fiber.