Recently, β-phase of calcium pyrophosphate has gained wide attention for potential in different applications. In this communication, we report for the first time an ultra-fast, cost-effective, and facile one-step synthesis of single-phase β-CPP powder without post-heat treatment by applying liquid flame spray (LFS). LFS is a scalable, continuous, and adjustable one-step flame-based aerosol synthesis method. The effect of Ca/P ratio on structural properties was investigated. β-Ca2P2O7 could be successfully synthesized in spherical nano-and micron-sized particles, as well as plate-like particles. The synthesized single-phase powder exhibited high thermal stability and relatively high specific surface area with different (nano)porous structures.