We investigate the entanglement between electronic and vibrational degrees of freedom produced by a vibronic coupling in a molecular system described in the Born-Oppenheimer approximation.Entanglement in a pure state of the Hilbert space H=H el H vib is quantified using the von Neumann entropy of the reduced density matrix and the reduced linear entropy. Expressions for these entanglement measures are derived for the 2 × N v and 3 × N v cases of the bipartite entanglement, where 2 and 3 are the dimensions of the electronic Hilbert space H el , and N v is the dimension of H vib . We study the entanglement dynamics for two electronic states coupled by a laser pulse (a 2 × N v case), taking as an example a coupling between the a 3 Σ + u (6s, 6s) and 1 g (6s, 6p 3/2 ) states of the Cs 2 molecule. The reduced linear entropy expression obtained for the 3 × N v case is used to follow the entanglement evolution in a scheme proposed for the control of the vibronic dynamics in a Cs 2 cold molecule, implying the a 3 Σ + u (6s, 6s), 0 − g (6s, 6p 3/2 ), and 0 − g (6s, 5d) electronic states, which are coupled by a non-adiabatic radial coupling and a sequence of chirped laser pulses.