Ever-growing various applications, especially for tissue regeneration, cause a pressing need for novel methods to functionalize melt electrowritten (MEW) microfibrous scaffolds with unique nanomaterials. Here, two novel strategies are proposed to modify MEW polycaprolactone (PCL) grids with ZnO nanoparticles (ZP) or ZnO nanoflakes (ZF) to enhance osteogenic differentiation. The calcium mineralization levels of MC3T3 osteoblasts cultured on PCL/ZP 0.1 scaffolds are ∼3.91-fold higher than those cultured on nonmodified PCL scaffolds, respectively. Due to the nanotopography mimicking bone anatomy, the PCL/ZF scaffolds (∼2.60 times higher in ALP activity compared to PCL/ZP 1 and ∼2.17 times higher in mineralization compared to PCL/ZP 0.1) achieved superior results. Moreover, the flexible feature inherited from PCL grids makes it possible for them to act as a reshapable osteogenic bioscaffold. This study provides new strategies for synthesizing nanomaterials on microscale surfaces, opening up a new route for functionalizing MEW scaffolds to fulfill the growing demand of tissue engineering.