In this research work, we investigated the effect of two cellulose nanocrystal (CNC)-related parameters, namely aspect ratio and loading content on the mechanical and desalination performance of a cellulose diacetate (CDA) model membrane system. Dispersion of high aspect ratio (HAR) CNCs in the CDA resulted in different types of nanoassembly, represented by evaluating the mechanical efficacy coefficient (C_FE), viscoelastic responses and separation performance of the nanocomposite membranes. Accordingly, 0.15 and 0.25 wt% showed random isolated dispersion and tight polymer-nanorod network, while 0.50 and 0.75 wt% conformed to nanorods' pervasive interconnected network (PIN) through side-by-side aggregation and intensive bundle alignment, respectively. Specifically, the nanocomposite membrane containing 0.50 wt% HAR-CNCs simultaneously demonstrated improved mechanical strength along with mitigated water permeability/salt rejection tradeoff for brackish water desalination. This concurrent boosting was attributed to the effective mechanical reinforcement mechanism induced by the percolating network along with its partial aggregation-caused bi-continuous and electrostatically-controlled nano-pathways, orchestrating the separation tradeoff. It confirmed our hypothesis that a nanocomposite membrane with metamaterial characteristic could be obtained via manipulating the dispersion state of CNC rods in the CDA, triggering coincided optimization of mechanical strength and desalination performance.