Host polymers play an important role in determining the thermal, optical and electrical properties of guest-host electro-optic (EO) polymers. In this study, a series of novel polymers, polyaryletherketones (PEKs) and polyarylethersulfones (PES'), were synthesized. After an initial screening on EO modulator fabrication-related properties, a PEK, LP120, was identified as a good candidate to host the highly stable chromophores (DH6 and DH52) developed in the company. Further optimization indicated that solvents in chromophore/polymer solutions have a strong impact on the quality of spin-coated films. DH6/LP120 and DH52/LP120 films spun from cyclopentanone gave lower optical losses of 1.97 and 1.55 dB/cm, respectively, when compared with 2.84 dB/cm for DH6/APC and 1.96 dB/cm for DH52/APC. Moreover, poling efficiencies as being reflected by EO coefficient were also improved by using LP120 compared to APC.