In this study, a new polymer P1 embedded with “H”-type chromophore moieties was designed and synthesized through Suzuki coupling copolymerization, in which the isolation chromophore was introduced to further improve its comprehensive performance. This polymer demonstrated good solubility and film-forming ability. In comparison with normal ”H”-shaped NLO polymers only containing one type of chromophore, nearly all the performance of P1 was improved. Its NLO coefficient was as high as 134 pm V−1, and its onset temperature for decay was up to 150 °C. Coupled with its improved optical transparency, all these properties made it a promising candidate for practical applications in photonic fields.