In this Letter, we propose a scheme for generation and control of the entanglement and arbitrary superposition states between molecular vibrational and rotational modes. We consider molecules in parahydrogen to be excited by linearly polarized chirped pulses in infrared and microwave frequency regions. From the calculations, it turns out that efficient control can be achieved. As a demonstration, we focus on HF and LiH molecules and clarify the effect of molecular characteristics on the state preparation using the molecular vibrational and rotational modes. (C) 2007 Elsevier B.V.. All rights reserved.