AbstractTitle compound,Mr=1273.16, was synthesized by a substitution reaction and its crystal is triclinic belonging to space groupP1with cell parameters:a=13.944(2),b=14.143(7),c=14.233(3) Å, α =77.35(3)°, β =69.94(2)°, γ =63.50(3)°,V=2351(1) Å3,Z=2,Dc=1.799g cm−2. Room temperature, graphite‐filtered Mo Kαradiation (λ =0.71073Å) was used for data collection. μ =14.988 cm−1,F(000) =1280,R=0.051 for 7025 observed reflections. The crystal consists of decrete cluster molecules containing a cluster core [Mo2(μ3‐S)]10+with three μ‐S, oneμ‐dtp(dtp =[S2P(OC2H5)]2‐), three χ‐dtp and one allylthioureo to form a local six‐coordinated sphere around each Mo atom. The bonds of cluster skeleton [Mo3(μ3‐S)(μ‐S)3]4+, MoMo 2.744∼2.766, Mo—(μ2‐S) 2.340∼2.342 and Mo—(μ‐S)2.272∼2.296 Å