A series of novel unsymmetrically disubstituted acylthioureas fused with hydrophenanthrene structure were synthesized from Δ⁸-dihydroabietic and dehydroabietic acid, respectively. Their structures were characterized by IR, ¹H-, and ¹³C-NMR spectroscopy. The antitumor activities of the title compounds against SMMC7721 and A549 tumor cells were evaluated by MTT (3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide) method. The results showed that three compounds (4c1, 4d1, and 4d2) exhibited highly effective activities against SMMC7721 and A549 cells, their IC₅₀ values are between 1.87–12.67 μM for SMMC7721 cells and 2.20–6.79 μM for A549 cells, respectively. Structure–activity relationship indicating that acylthioureas that furan group fused with Δ⁸-dihydroabietyl group, trihydroxymethyl fused with Δ⁸-dihydroabietyl and dehydroabietyl could generate enhance activities of this kind of compounds against SMMC7721 and A549 cells.