This study reports dicarboxylate cellulose nanofibrils (DCNF) as a novel reducing and supporting agent for producing silver nanoparticles (AgNPs) with high efficiency (63.82 % reduction) and loading (6.88 %) using UV light. Unlike previous research, AgNPs formation with DCNF doesn't involve cellulose oxidation. Instead, it appears to involve a loss of carboxyl groups from DCNF. In comparative studies, pristine CNF (PCNF) and TEMPO-oxidized CNF (TOCNF) were also examined for AgNPs production. The resulting AgNPs from DCNF exhibited a significantly smaller average size (3.9 ± 0.7 nm) compared to those from PCNF (26.9 ± 10.9 nm) and TOCNF (13.5 ± 4.5 nm). Catalytic activity evaluation by the 4-nitrophenol (4-NP) reduction reaction revealed a high rate constant of 8.47× 10−3 s−1 by AgNPs/DCNF, which surpassed AgNPs/TOCNF (1.79 × 10−3 s−1) and AgNPs/PCNF (0.63 × 10−3 s−1) by 4.7 and 13.4 times, respectively. Besides 4-NP, AgNPs/DCNF aerogels were also applied for methyl orange and Rhodamine B dyes reduction. The aerogels showed excellent reusability, maintaining over 95 % conversion even after five cycles and also effective in treating real samples and mixed dye solutions. This study opens the door for future research exploring DCNF as a support material for various metal, metal oxide, and carbon nanoparticles.