Polylactide/hydroxyapatite (PLA/HA) composites are promising tissue engineering materials because of the PLA biodegradability and HA as a natural bone component. PLA/HA composites without HA modification lead to mechanical failure due to the interfacial immiscibility. In this study, an effective chemical surface methodology is used to modify HA to obtain PLA/HA composites with superior mechanical properties. The HA particles are modified with fatty acids (adipic, sebacic, lauric, and linoleic) and incorporated into a PLA matrix by polymer solution casting, using chloroform as the solvent. After the HA modification, the films exhibited an improvement in tensile strength, elongation at break, and elastic modulus. Yet, the best results observed are by sebacic and adipic acid modification. These increments are attributed to a higher affinity of the organo‐modified HA particles within the PLA matrix. Therefore, the development of materials for osteo‐regeneration engineering based on these systems is quite promising.