The development of biohybrid materials combining metal–organic frameworks (MOFs) and biopolymers has emerged as a promising strategy to enhance material performance in water purification applications. In this work, we report the synthesis and morphological characterization of zeolitic imidazolate framework-8 (ZIF-8)/nanocellulose hybrid materials. High-resolution scanning electron microscopy (SEM) reveals that ZIF-8 nanocrystals are embedded within cellulose nanofiber (CNF) networks, where the high aspect ratio of the nanofibers facilitates physical bridging between individual ZIF-8 particles. Notably, phosphorylated CNFs (phos-CNFs) exhibit thinner, more individualized fibers compared to unmodified CNFs, which form dense nanofiber bundles, likely due to enhanced hydrogen bonding. These structural differences impact the biohybrid morphology, influencing the size of ZIF-8 crystals formed within the network, with phos-CNF hybrids producing larger particles (495.15 ± 143.74 nm) relative to those templated by unmodified CNFs (150.19 ± 30.68 nm). Furthermore, cellulose nanocrystals (CNCs) display unique facet-selective interactions with ZIF-8, assembling preferentially on specific crystal planes. To complement morphological studies, atomic force microscopy (AFM) will be employed to investigate the nanomechanical properties of these hybrids and quantify the interaction forces at the interface. Together, these insights provide a multiscale understanding of ZIF-8/nanocellulose assembly and offer valuable design principles for advanced biohybrid materials in environmental remediation.