Two formulas of grafted polymers with metal-containing chromophores, potentially suitable for second-order nonlinear optics applications, are described. Two chromophores were obtained from a tridentate ligand coordinated to Cu(II) or Pd(II) ions. The organometallic chromophore fragments were grafted to poly(4-vinylpyridine) by the pyridinic nitrogen of the host polymer. Some qualities displayed by the new metallated polymers are remarkable: (1) a high value of the first hyperpolarizability coefficient of the chromophores, (2) a high content of the grafted chromophore in the polymers (up to 60 wt %), (3) a considerable increase in the glass-transition temperatures (up to 240 degreesC), (4) good thermal stability in air (ca. 280 degreesC), and (5) good optical transparency of the films.