The first evidence of spin alignment of vector mesons ($K^{*0}$ and $\phi$) in heavy-ion collisions at the Large Hadron Collider (LHC) is reported. The spin density matrix element $\rho_{00}$ is measured at midrapidity ($|y| <~$ 0.5) in Pb-Pb collisions at a center-of-mass energy ($\sqrt{s_{\rm NN}}$) of 2.76 TeV with the ALICE detector. $\rho_{00}$ values are found to be less than 1/3 (1/3 implies no spin alignment) at low transverse momentum ($p_{\rm T} <~$ 2 GeV/$c$) for $K^{*0}$ and $\phi$ at a level of 3$\sigma$ and 2$\sigma$, respectively. No significant spin alignment is observed for the $K^0_S$ meson (spin = 0) in Pb-Pb collisions and for the vector mesons in $pp$ collisions. The measured spin alignment is unexpectedly large but qualitatively consistent with the expectation from models which attribute it to a polarization of quarks in the presence of angular momentum in heavy-ion collisions and a subsequent hadronization by the process of recombination.