In this study, we report the growth of surfactant‐free silver nanoparticles (NPs) on cotton through a facile chemical reduction method, iteratively applied to gradually increase and control the concentration of silver NPs. Our substrates showed enhanced performance in surface enhanced Raman spectroscopy (SERS), catalytic, and antibacterial properties, all attributable to the high concentration of NPs on the cotton and their surfactant‐free nature. While the antibacterial properties improve with increasing growth cycles, SERS and catalytic properties first increase from the first to fourth growth cycles and then decrease for the fifth growth cycle. For substrate with optimum deposition for SERS, rhodamine 6G (R6G) analyte down to nanomolar concentrations were detectable, with a linear correlation of intensity versus concentration and exhibit excellent uniformity in the SERS signal. Furthermore, the catalytic activity of our substrates against the degradation of methyl orange (MO) was impressive with a rate constant of 0.0866 min−1 for the first growth cycle, which increased by ~3.4‐fold to 0.2979 min−1 for the fourth growth cycle. Finally, the substrates showed excellent antibacterial activity towards both Gram‐negative (E. coli) and Gram‐positive (S. aureus) bacteria. For both bacteria, the zone of inhibition increased with increasing growth cycles.