This study presents a novel, green, and efficient way of preparing crosslinked aerogels from cellulose nanofibers (CNFs) and alginate using non-covalent chemistry. This new process can ultimately facilitate the fast, continuous, and large-scale production of porous, light-weight materials as it does not require freeze-drying, supercritical CO2 drying, or any environmentally harmful crosslinking chemistries. The reported preparation procedure relies solely on the successive freezing, solvent-exchange, and ambient drying of composite CNF-alginate gels. The presented findings suggest that a highly-porous structure can be preserved throughout the process by simply controlling the ionic strength of the gel. Aerogels with tunable densities (23–38 kg m−3) and compressive moduli (97–275 kPa) can be prepared by using different CNF concentrations. These low-density networks have a unique combination of formability (using molding or 3D-printing) and wet-stability (when ion exchanged to calcium ions). To demonstrate their use in advanced wet applications, the printed aerogels are functionalized with very high loadings of conducting poly(3,4-ethylenedioxythiophene):tosylate (PEDOT:TOS) polymer by using a novel in situ polymerization approach. In-depth material characterization reveals that these aerogels have the potential to be used in not only energy storage applications (specific capacitance of 78 F g−1), but also as mechanical-strain and humidity sensors. © 2020 The Authors.