Dolomite, a prevalent mineral in rock formations, often coexists with various minerals, impacting their properties and typically being discarded as waste in the extraction process of other minerals. This research introduces a straightforward and effective technique for co-calcining urea with natural dolomite at 550℃, yielding a novel composite adsorbent designated as CN/xDO, where ‘x’ denotes the proportion of dolomite incorporated. During the preparation, urea promotes the conversion of dolomite to nano calcite, and the gas produced by urea pyrolysis during the calcination process has a cavitation effect on the material, enhancing its surface properties. BET analysis reveals that the specific surface area and total pore volume of CN/xDO notably surpass those of pure dolomite, with CN/0.6DO achieving 2.9479 m2/g and 0.0382 cm3/g, respectively. CN/0.6DO demonstrates an adsorption capacity of 237.91 mg/g for La(III) within 360 min at 298 K, which is 16.9 times greater than that of untreated dolomite (14.05 mg/g). The maximum adsorption capacity of CN/0.6DO for La(III) (C0 = 500 mg/L) reaches 382.94 mg/g at 308 K, exceeding the majority of adsorbents documented in the literature. The comparative analysis of batch adsorption experiments and material characterization before and after the adsorption process reveals that the mechanisms adsorption of La(III) adsorption by CN/xDO include physical adsorption, cation-π interactions, ion exchange, and complexation with oxygen-containing functional groups, especially −OH, CO32-. This study broadens the application of dolomite in adsorption and introduces a new strategy for the efficient recovery of rare earth elements from wastewater, consistent with the principles of sustainable development.