A clear understanding of the temperature evolution of the longitudinal spin Seebeck effect (LSSE) in the classic Pt/yttrium iron garnet (YIG) system and its association with magnetic anisotropy is essential towards optimization of its spin-caloric functionality for spintronics applications. We report here for the first time the temperature dependences of LSSE voltage (V LSSE ), magnetocrystalline anisotropy field (H K ) and surface perpendicular magnetic anisotropy field (H KS ) in the same Pt/YIG system. We show that on lowering temperature, the sharp drop in V LSSE and the sudden increases in H K and H KS at ~175 K are associated with the spin reorientation due to single ion anisotropy of Fe 2+ ions. The V LSSE peak at ~75 K is attributed to the H KS and M S (saturation magnetization) whose peaks also occur at the same temperature. The effects of surface and bulk magnetic anisotropies are corroborated with those of thermally excited magnon number and magnon propagation length to satisfactorily explain the temperature dependence of LSSE in the Pt/YIG system. Our study also emphasizes the important roles of bulk and surface anisotropies in the LSSE in YIG and paves a new pathway for developing novel spincaloric materials.Spin caloritronics based on the spin-Seebeck effect (SSE) is an emerging area of research owing to its potential use in advanced spintronics devices 1,2 . SSE is associated with the generation of pure spin current without charge current when a thermal gradient is established in the presence of an applied magnetic field 3 . Since the discovery of SSE in a ferromagnetic metal (NiFe), it has been reported in a wide range of materials, including ferromagnetic insulators, ferromagnetic semiconductors, and non-magnetic materials, using longitudinal and transverse measurement configurations (known as LSSE and TSSE, respectively) [3][4][5][6][7] . The great diversity of host materials raises an important question about the underlying physical origin of the SSE [8][9][10][11] . In particular, the origin of the temperature dependence of the LSSE in the Pt/YIG system has been a subject of long lasting debate 9 . Siegal et al. observed a decrease in the LSSE voltage (V LSSE ) with decreasing temperature in Bi-YIG thin films, with a sudden change of V LSSE slope below 200 K 11 . While the origin of the sudden change in V LSSE below 200 K was unclear 11 , this may be associated with spin reorientation due to single ion anisotropy of Fe 2+ ions that was also reported to occur below 200 K in the single crystalline YIG 12 . It has recently been reported that when the thickness of YIG exceeds its magnetic domain size (~5 μm), the magnetic field-dependent V LSSE shows an anomaly in a low field regime (<±0.3 kOe) 13 . This low field feature has been attributed to the presence of an intrinsic easy axis perpendicular magnetic anisotropy (PMA) at the YIG surface 13 . The presence of PMA has been experimentally shown at 300 K to influence the value of the saturation magnetic field H ( ) . These experimental observ...