Digital printing waste paper fiber/nano-crystalline cellulose/poly (lactic acid) (DPF/NCC/PLA) composites, modified through γ-methacryloxy propyl trimethoxy silane (KH570), isopropyl tri (dioctylpyrophosphate) titanate (TMC201), sodium hydroxide (NaOH), polyethylene glycol 6000 (PEG6000), and a composite silane coupling agent (KH570/PEG6000), were fabricated by melt blending and injection molding and the effects of different modifiers on the properties of composites were studied. Results showed that mechanical properties of the modified composites generally improved, and the best mechanical properties, including flexural, tensile and impact strength, were achieved PEG6000, KH570/PEG6000, and KH570 modification, respectively. Thermal performance analysis showed improved thermal properties of composites treated by KH570, but the crystallinity of the modified materials was increased. Both water absorption and degradation properties showed a decreasing trend, and water absorption performance was obviously improved after KH570/PEG6000 modification. Under the action of several modifiers, the diffusion coefficient, thermodynamic solubility and permeability of composites were reduced to varying degrees. Furthermore, scanning electron microscopy (SEM) demonstrated that interfacial adhesion and composite compatibility were improved with significantly fewer and smaller pores, as well as a fuzzy boundary among the three phases.