Wood fiber of aspen was used as a reinforced filler in linear low-density polyethylene (LLDPE). To improve the compatibility between the wood fiber and the LLDPE matrix, the wood fiber was treated with titanate coupling agents (i.e., TC-PBT and TC-POT) or grafted by acrylonitrile. Both treatments resulted in an improvement in the mechanical properties of the resultant composites compared with the composites filled with the untreated wood fiber. Moreover, the grafting method displayed a more obvious benefit than that of titanate coupling methods to the mechanical property improvement. This was attributed to the crystalline structure of the wood fiber to be destroyed by grafting acrylonitrile, and the amorphous fiber was easily deformed to enhance fiber adhesion at the LLDPE matrix. In addition, the effect of the concentration of the filled wood fiber and the amount of coupling agent or grafting ratio on the mechanical properties of composites are discussed.