Layered two-dimensional conjugated polymers (2D CPs), or 2D conjugated covalent organic frameworks, are promising semiconductor materials for (opto)electronics and photocatalysis, but their performance is often limited by insufficient in-plane conjugation and poor charge transport. Guided by density functional theory calculations, we report two donor-acceptor-type 2D poly(arylene vinylene)s constructed from thienyl-benzodithiophene and diketopyrrolopyrrole units. These materials are predicted to exhibit strongly dispersive energy bands with ultralow in-plane effective masses (0.036 − 0.159 m₀), enabling intrinsic charge mobilities approaching 2000 cm²V⁻¹ s⁻¹. Solid-state Aldol-type 2D polycondensation yields crystalline materials with optical band gaps as narrow as 1.0 eV. Terahertz spectroscopy reveals long charge carrier scattering times of 76 fs and a high room-temperature mobility of 310 cm²V⁻¹ s⁻¹, surpassing previously reported linear and 2D CP powder samples. This work highlights donor-acceptor engineering as an effective strategy to enhance charge transport in 2D CPs.