Oil palm empty fruit bunches (OPEFB) is waste from crude palm oil (CPO) processing plants. This research aims to process OPEFB to be a reinforcement polymer recycle with the mechanical milling method and identify each establishment molecular with the orbital hybridization theory. OPEFB fibers were synthesized using a mechanical milling until the size shortfiber and microfiber. Then do the biocomposite granular synthesis with single screw extruder. TAPPI chemical test shows levels of α-cellulose fibers amounted 41.68%. Based on density, the most optimum composition contained in the filler amounted 15% with the size is the microfiber. The test results of morphology with SEM showed deployment of filler OPEFB fiber is fairly equitable distributed. Regarding the molecular interaction between matrix with OPEFB fiber, described by the theory of orbital hybridization. But the explanation establishment of the bond for more complex molecules likes this from the side of the molecular orbital theory is necessary complete information of the hybrid levels.