Natural fiber composite materials are widely used in various structural fields, interior design, and sports equipment in the present scenario because of their high specific strength, stiffness and biodegradability properties. Various applications in these emerging fields induce the manufacturers to examine its tribological performance. This work deals with the development and erosion wear characteristics of giant-cane (Arundinaria gigantea) fiber-reinforced filled nanozirconia toughened mullite (ZTM) epoxy composite. The three-layered composite laminate is fabricated by hand lay-up technique using woven cellulosic giant-cane fiber mat, epoxy resin and ZTM nano-filler. Three different types of specimen are fabricated by varying weight percentages of ZTM filler as 0, 5 and 10. Angle-ply [+ 45°/− 45°/ + 45°] configured specimens are fabricated and tested to study the erosion wear behavior of composite specimens. The test is carried out by taking the parameters such as impact velocity, impingement angle and filler content by adopting Research Surface Methodology (RSM). The erosion wear test revealed that the impact velocity, impingement angle and contents of filler influence the wear characteristics of giant-cane fiber composite. Further, the impact velocity and impingement angle play significant role in determining the erosion rate. The impact velocity of 40 m/s, impingement angle at 45° and filler percentage of 10% bears the minimum erosion rate which is predicted to be 109.26 mg/k.