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Catalytic dechlorination of organic chlorides by palladium (Pd) with HCOOH represents one of the most effective and promising techniques for environmental remediation. In this study, we adopted alkaline-modified porous natural sponge as support of a Pd nanocatalyst (Pd@M-Sponge) and HCOOH as a hydrogen source for the hydrodechlorination of florfenicol (FF), <i>o</i>-chlorophenol (<i>o</i>-CP), and <i>p</i>-chlorophenol (<i>p</i>-CP). Favorable conversion efficiency of FF, <i>o</i>-CP, and <i>p</i>-CP was achieved at 25 °C and atmospheric pressure attributed to the small diameter and high catalytic reactivity of the prepared Pd NPs, in addition to the slight internal mass transfer limitation of the prepared Pd@M-Sponge. High reaction rate constants were obtained even in the conditions of a low molar ratio of HCOOH to <i>p</i>-CP (10:1) and a high concentration of <i>p</i>-CP (500 mg/L). The prepared catalyst also demonstrated superior recyclability without any obvious decrease in catalytic reactivity in 20 successive <i>p</i>-CP dechlorination cycles. This work provides an ideal recyclable and cost-effective catalyst based on renewable and biocompatible natural material for the catalytic hydrodechlorination of chlorinated organic pollutants with formic acid and a new view for the exploration and designing of highly reactive and stable catalysts for hydrodechlorination.