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Calcium alginate (Ca-Alg) is a novel target product for recovering alginate from aerobic granular sludge. A novel Ca-Alg production method was proposed herein where Ca-Alg was formed in a sodium alginate (SA) feed solution (FS) and concentrated via forward osmosis (FO) with Ca²⁺ reverse osmosis using a draw solution of CaCl₂. An abnormal reverse solute diffusion was observed, with the average reverse solute flux (RSF) decreasing with increasing CaCl₂ concentrations, while the average RSF increased with increasing alginate concentrations. The RSF of Ca²⁺ in FS decreased continuously as the FO progressed, using 1.0 g/L SA as the FS, while it increased initially and later decreased using 2.0 and 3.0 g/L SA as the FS. These results were attributed to the Ca-Alg recovery production (CARP) formed on the FO membrane surface on the feed side, and the percentage of Ca²⁺ in CARP to total Ca²⁺ reverse osmosis reached 36.28%. Scanning electron microscopy and energy dispersive spectroscopy also verified CARP existence and its Ca²⁺ content. The thin film composite FO membrane with a supporting polysulfone electrospinning nanofiber membrane layer showed high water flux and RSF of Ca²⁺, which was proposed as a novel FO membrane for Ca-Alg production via the FO process with Ca²⁺ reverse diffusion. Four mechanisms including molecular sieve role, electrification of colloids, osmotic pressure of ions in CARP, and FO membrane structure were proposed to control the Ca-Alg production. Thus, the results provide further insights into Ca-Alg production via FO along with Ca²⁺ reverse osmosis.