Poly(L-lactic acid) (PLLA) micro-fibers have been coated with hydroxyapatite (HA) using a quick biomimetic method to form a precursor for bone repair composites. To increase the coating content within a coating time as short as 1–2.5 h, PLLA fibers have been treated by soaking in NaOH or NaOCl solutions at mild conditions. Although different surface hydrolysis and coating methods have been used to prepare bioceramic/polymer composites, it is for the first time that the influences of the surface treatment and HA coating process on the mechanical properties of the polymer and HA/polymer composite fibers were investigated systemically.