In order to derive a possible direction for developing Reynolds-averaged algebraic turbulent scalar-flux models, a priori explorations are attempted by processing the LES data presently performed for channel flows under several flow-boundary conditions including shear-free boundaries. The present calibration has elucidated that the turbulent scalar-flux vectors obtainable from the simple generalized gradient-diffusion hypothesis (GGDH) hardly align with the simulation results in wall-shear flows at Pr greater than or equal to 0.71. However, the GGDH form returns a quite reasonable approximation in shear-free flow regions and/or lower Pr fluid cases. In the former flow cases, it has been found that an introduction of quadratic products of the Reynolds-stress tensor into the gradient diffusion model may improve the predictive performance. (C) 2001 Elsevier Science Inc. All rights reserved.