Hydrogen-substituted graphyne (HsGY) composed of alternative phenylene and ethynylene units were synthesized with organic solvents and deep eutectic solvents as reaction solvents by cross-coupling polymerization of 1, 3, 5- triethynylbenzene and 1, 3, 5-tribromobenzene. The microstructure and properties of HsGYs were analyzed by various characterization methods. Sphere, reticular, irregular massive, claws-like, fibrous structures were observed by scanning electron microscope using the mesitylene, N, N-dimethylformamide and three DESs, respectively. The results showed that the morphologies of five HsGYs were greatly affected by the choice of solvents. The chemical structure of the HsGYs was confirmed by Fourier transform infrared spectroscopy and solid-state 1H magic-angle spinning nuclear magnetic resonance. Moreover, HsGYs with different morphologies had chemical stability, high thermal stability, super-hydrophobic, and semiconductor properties. Studies had shown that HsGY-D (N, N-dimethylformamide as solvent) with the largest specific surface area (1453.16 m2 g−1) and average pore diameter (40.10 Å) had the strongest adsorption performance for carbendazim and thiabendazole by static adsorption test in dried jujube sample. This work was expected to provide useful guidance to rationally design alkynyl carbon materials in adsorption of organic chemical pollutants.