The removal of harmful cyanobacterial blooms (HCBs) and reuse of the resulting algal sludge are pressing issues in current environmental governance and ecological conservation. Aiming at tackling the above-mentioned challenges, titanium (Ti)-based coagulants are promising candidates. However, most of them suffer from poor stability and weak actual algal removal ability, and recycling of the algal sludge usually produces titanium dioxide (TiO2) with low photocatalytic ability. In this work, a lanthanum (La)-modified polytitanium chloride (La-PTC) coagulant is reported. La in the La-PTC coagulant serves a "kill two birds with one stone" strategy in algae removal and algae sludge reuse. Owing to the introduction of La ions, the La-PTC coagulant exhibits ultra-high stability and excellent algae removal capability with an efficiency of 98.71%, which is 7.25% higher than that of PTC coagulant. Moreover, recycling algae sludge can prepare high catalytic (2.45 times the commercial P25 TiO2) La/C-TiO2, where the presence of La enhances its visible light response range and inhibits electron hole recombination. The strategy of this La modified coagulant can not only achieve efficient removal of HCBs, but also transform the recovered algal sludge into photocatalysts with higher catalytic capacity.