One of strongly “pi-d” interacting systems in organic material is lambda-(STF)2MCl4 (M= Fe, Ga) (STF is C10S6Se2H8: bisethylenedithiodiselenadithiafulvalene). Ga compound doesn’t have d-spin and it is a good target to study a pure pi spin properties in the conduction band of the STF two-dimensional sheet. It is a pressure induced superconductor above 1.2 GPa with Tc~5 K. At ambient pressure, it shows insulating phase which we expect that it is a quantum spin liquid candidate from our NMR and susceptibility data down to 1.6 K. If we change Ga to Fe which has 3d spin, it shows antiferromagnetic ordering at 16 K, evidenced by our NMR data. But the effect from d-spin to p-spin (ordering?) is not experimentally clarified yet. We want to study how spin liquid-like behavior in Ga compound is broken by introducing d-spin in Fe compound, which competes with pi-spin, by ZF and LF muSR.