Hydrophilic behaviour of carrageenan macroalgae biopolymer, due to hydroxyl groups, has limited its applications, especially for packaging. In this study, macroalgae were reinforced with cellulose nanofibrils (CNFs) isolated from kenaf bast fibres. The macroalgae CNF film was after that treated with silane for hydrophobicity enhancement. The wettability and functional properties of unmodified macroalgae CNF films were compared with silane-modified macroalgae CNF films. Characterisation of the unmodified and modified biopolymers films was investigated. The atomic force microscope (AFM), SEM morphology, tensile properties, water contact angle, and thermal behaviour of the biofilms showed that the incorporation of Kenaf bast CNF remarkably increased the strength, moisture resistance, and thermal stability of the macroalgae biopolymer films. Moreover, the films’ modification using a silane coupling agent further enhanced the strength and thermal stability of the films apart from improved water-resistance of the biopolymer films compared to unmodified films. The morphology and AFM showed good interfacial interaction of the components of the biopolymer films. The modified biopolymer films exhibited significantly improved hydrophobic properties compared to the unmodified films due to the enhanced dispersion resulting from the silane treatment. The improved biopolymer films can potentially be utilised as packaging materials.