We demonstrate the interplay of pure spin current, spin-polarized current, and spin fluctuation in 3d Ni_{x}Cu_{1-x}. By tuning the compositions of the Ni_{x}Cu_{1-x} alloys, we separate the effects due to the pure spin current and spin-polarized current. By exploiting the interaction of spin current with spin fluctuation in suitable Ni-Cu alloys, we obtain an unprecedentedly high spin Hall angle of 46%, about 5 times larger than that in Pt, at room temperature. Furthermore, we show that spin-dependent thermal transport via anomalous Nernst effect can serve as a sensitive magnetometer to electrically probe the magnetic phase transitions in thin films with in-plane anisotropy. The enhancement of spin Hall angle by exploiting spin current fluctuation via composition control makes 3d magnets functional materials in charge-to-spin conversion for spintronic application.