Interphase Engineering in Lignin-Containing Nanocellulose Composites from Tropical Biomass: Evidence-Weighted Comparative Framework, Product Windows, and Biorefinery Constraints

Tropical lignocellulosic residues are increasingly relevant feedstocks for lignin-containing nanocellulose composites, but their performance cannot be predicted from botanical origin or bulk lignin percentage alone. This review defines the interface as the geometrical boundary between phases and the interphase as the finite, compositionally graded region in which lignin distribution, nanocellulose morphology, adsorbed water, and the surrounding matrix jointly govern stress transfer and mass transport. Using an evidence-weighted framework, the literature is organized into the following categories: residual-lignin nanofibrils, redeposited-lignin systems, lignin nanoparticle assemblies, compatibilized thermoplastic hybrids, and all-lignocellulosic sheets. Representative quantitative observations show that controlled residual lignin can the increase water contact angle from approximately 35 degrees to 78 degrees and reduce oxygen permeability by up to 200-fold in nanopapers, while selected PLA/LCNF systems show tensile-strength and modulus increases of 37% and 61%, respectively; however, high or poorly distributed lignin can suppress fibrillation, lower viscosity, weaken gel networks, and reduce reproducibility. The most defensible near-term product windows are packaging layers, grease/oil barrier papers, coatings, paper-like multilayers, and selected porous media. Thermoplastic matrices remain process-sensitive, and biomedical, additive-manufacturing, nano-reactor, and energy-material claims require stronger validation of the extractables, rheology, humidity history, TEA/LCA metrics, and end-of-life behavior. This review, therefore, provides a critical, application-backward roadmap for tropical biorefineries in which interfacial function, wet handling, drying energy, and process integration are assessed together rather than treated as independent variables. The abbreviations used in the abstract are defined as follows: CNFs, cellulose nanofibrils; CNC, cellulose nanocrystals; LCNF, lignin-containing cellulose nanofibrils; LCNCs, lignin-containing cellulose nanocrystals; PLA, poly(lactic acid); PHB, polyhydroxybutyrate; PHAs, polyhydroxyalkanoates; PVA, poly(vinyl alcohol); DESs, deep eutectic solvents; TEA, techno-economic analysis; LCA, life-cycle assessment; ML, machine learning.