(1) Phosphorus (P) removal has proven difficult in decentralized wastewater treatment systems, and P binding material, installed as an external filter, has been proposed for improving P removal. Especially, calcium (Ca)-rich materials have shown promising results. (2) Five calcareous materials were tested with isotherm batch experiments. The material with the highest P adsorption capacity was selected to undergo different Sol-Gel coatings, i.e., different coating dilution ratios (1:10, 1:5, and 1:1) and exposure periods (5, 10, and 15 min). The seven coated materials were evaluated by isotherm experiments. (3) The maximum adsorption capacity (Qmax) was determined by fitting the Langmuir equation. Qmax for the non-coated materials, and ranged from 0.7 (sand) to 35.1 (Catsan) mg P g−1 DW, while the coated materials ranged from 7.8 to 24.7 mg P g−1 DW depending on the coating. Based on the rotated Principal Component Analysis, the most important parameters for Qmax were the texture and the Ca content. (4) Catsan was the most promising material, but when performing a Sol-Gel coating, a trade-off between preserving Qmax and the coating thickness were evident, as the materials with the thinner coating preserved more of the sorption capacity. The development of P binding materials constitutes a useful technology in decentralized wastewater treatment systems.