Food-waste-derived bio-based materials offer both environmental and economic advantages. We utilised waste lemon peel as substrate to generate value-added materials from chitosan-rich fungal cell wall of Rhizopus delemar and purified cellulose from pre-treated solid residues. Nutrient from lemon peel was used for fungal cultivation and the cell wall was isolated from the obtained fungal biomass using mild alkali treatment. The fungal cell wall was used to develop a hydrogel through protonation of amino groups in chitosan by lactic acid addition. This hydrogel served as spinning dope to produce fungal monofilaments using dry gel spinning with a tensile strength of 85 MPa. Simultaneously, cellulose purified from pre-treated solid residues, converted to micro-nanocellulose suspension via mechanical fibrillation and underwent dry gel spinning to produce cellulose monofilaments with a tensile strength of 298 MPa. Cellulose fraction was analysed using XRD, FTIR, TGA, and elemental analyses. The micro- and nanoscale structures of fibrillated cellulose were verified by SEM and AFM. The findings of this study demonstrate a novel holistic valorisation approach for lemon peel waste as a resource for bio-based monofilaments, which could be used as alternatives to commercial fibres in textiles.