The current study aims to examine the influence of surface‐modified micro‐sized walnut shell particulates (WSP) with an aqueous solution of sodium hydroxide (NaOH) on epoxy composites. For that, epoxy/WSP composites are prepared by varying the WSP content up to 20 wt%. In this investigation, the physical properties (surface morphology, density, voids percentage, water uptake), mechanical properties (tensile, flexural, compressive, hardness), and sliding wear behavior of the composites are reported. From the micrographs, it is clear that WSP established good adhesion with the epoxy matrix. Further, it is found that the density, void content, water intake capacity, compressive strength, and hardness increase with WSP loading. Against that, the tensile and flexural strength is somewhat reduced at higher filler loading. Sliding wear tests are performed as per L25 Taguchi's orthogonal array. From the analysis, it is observed that WSP content is the most significant factor and sliding distance is the least significant factor for minimizing the wear rate. For analyzing the sliding wear performance under varied conditions, a prediction model is proposed using an artificial neural network to forecast the sliding wear rate of epoxy/WSP composites over a wide range of experimental domains.