  Crystal structures of $\textrm{CLi}_4$ compounds are explored through
\emph{ab} \emph{initio} evolutionary methodology. Phase transition from metal
to semimetal and semiconductor, and eventually to insulator with increasing
pressure are revealed under pressure. Pressure-induced evolution of
anti-metallization has been described quantitatively by Fermi Surface Filling
Ratio and electron energy band gap using \emph{ab} \emph{initio} \emph{GW}
calculations. Anti-metallization is attributed to the hybrid valence electrons
and their repulsion by core electrons into the lattice interstices. Very weak
electron-phonon coupling interactions are found in the metallic phases,
resulting in very low superconducting temperature.
