We observe the process ψð3686Þ → ppη 0 for the first time, with a statistical significance higher than 10σ, and measure the branching fraction of J=ψ → ppη 0 with an improved accuracy compared to earlier studies. The measurements are based on 4.48 × 10 8 ψð3686Þ and 1.31 × 10 9 J=ψ events collected by the BESIII detector operating at the BEPCII. The branching fractions are determined to be Bðψð3686Þ → ppη 0 Þ ¼ ð1.10 AE 0.10 AE 0.08Þ × 10 −5 and BðJ=ψ → ppη 0 Þ ¼ ð1.26 AE 0.02 AE 0.07Þ × 10 −4 , where the first uncertainties are statistical and the second ones systematic. Additionally, the η − η 0 mixing angle is determined to be −24°AE 11°based on ψð3686Þ → ppη 0 , and −24°AE 9°based on J=ψ → ppη 0 , respectively.