Seaweed from macroalgae and cellulose from nonwood materials have gained attention in various fields. This study explores how seaweed and cellulose nanofibers (CNF) interact to form 3D networks in composite bioaerogels. The ratio of CNF and seaweed was varied to see how it affects the aerogel’s inside and its properties. The observations show that the biocomposite aerogel is more rigid and shrinks less than using a single biopolymer. The CNF aerogel has a fine, thin network structure, and the seaweed aerogel has a thin sheet structure. The biocomposite aerogel combines both a fine network and a thin sheet structure. The composite aerogel’s mechanical properties are significantly influenced by seaweed composition. The introduction of CNF increases elasticity, while seaweed enhances firmness. Generated computer modelling revealed that the abundant hydroxyl groups in CNF facilitated the formation of intermolecular bonds with seaweed. The bonding led to increased adhesion and entanglement between biopolymers, consequently enhancing elasticity and establishing a stable intermolecular interaction. The 3D X-ray imaging model shows that the skeletal framework primarily consists of seaweed biopolymer, with CNF serving to reinforce this structure thus enhancing the mechanical properties and robustness of the composite bioaerogels.