AbstractHot compression molding was used to produce biocomposites from ramie plain‐woven fabric‐reinforced polylactic acid (PLA). Prior to composite fabrication, alkali and dipodal silane (bis(3‐trimethoxysilylpropyl) amine) (BAS) were applied to improve fiber‐matrix adhesion. Mechanical tests revealed improvements in tensile and flexural strength due to interfacial adhesion. The flexural strength of ramie PLA composite samples treated only with silane (SR‐PLA) was the highest, at 136.35 MPa. Young's modulus was 7.51 GPa. BAS treatment was crucial for ensuring strong adhesion between the fabric and the PLA matrix. In combined alkali‐BAS‐treated composites (ASR‐PLA), the glass transition and crystallization temperatures disappeared completely, affecting PLA morphology. The maximum heat of absorption (373°C) was found in SR‐PLA composites, suggesting electrostatic interactions created a three‐dimensional network. In conclusion, the initial incorporation of dipodal silane resulted in the formation of six silanol linkages with ramie fabric, leading to enhancements in the mechanical and thermal characteristics of ramie–PLA composites.Highlights Alkali and BAS treated Fabrics ironed to remove treatment‐induced wrinkles. Carded PLA fiber with consistent density and weighted in four equal portions. Fabric and PLA lay alternatively in warp direction before compression molding. SR‐PLA composites exhibited improved thermal and mechanical properties.