Activity-guided fractionation of Erythrophleum succirubrum for TRAIL resistance-overcoming activity led to the isolation of four new cassaine diterpenoid dimers, named erythrophlesins A–D (1–4). Their structures were elucidated by spectral data to show that they have an unsymmetrical dimeric structure through an ester bond between two cassaine diterpenoids. These new compounds were revealed to have a significant reversal effect on TRAIL resistance in human gastric adenocarcinoma (AGS) cells.