We listed all possible dimension-six CP-violating \(SU_c(3)\times SU_L(2)\times U_Y(1)\) invariant operators involving the third-family quarks, which can be generated by new physics at a higher energy scale. The expressions of these operators after electroweak symmetry breaking and the induced effective couplings \(Wt\bar b\), \(Xb\bar b\) and \(Xt\bar t\) \((X=Z,\gamma,g,H)\) are also presented. We have evaluated sample contributions of these operators to CP-odd asymmetries of transverse polarization of top quark in single top production at the upgraded Tevatron, the similar effect in top-antitop pair production at the NLC, and the CP-odd observables of momentum correlations among the top quark decay products at the NLC. The energy and luminosity sensitivity in probing these CP-violating new physics has also been studied.