This study was conducted to investigate the accuracy of predicting in vitro ruminal methane (CH₄) production using  volatile fatty acids (VFA) stoichiometric models \[CH₄=0.5Ace-0.25Pro+0.5But-0.25Val\] (model 1), where CH₄, Ace, Pro, But and Val are the production amounts of CH₄, acetate, propionate, butyrate and valerate, respectively. Ten common feedstuffs, including four concentrates and six roughages with a wide range of  chemical composition were incubated in serum bottles, and VFAs and CH₄ production at 72 h were determined. The differences between the predicted and measured CH₄ production were quantified using the model accuracy analysis. The results showed that the predicted CH₄ production amounts were generally greater than the measured values obtained using the model 1, and the bias, slope and random error were 62.6%, 11.7% and 25.7%, respectively, indicating that fixed error exceeded 70%. By assuming 80% of total hydrogen being used for CH₄ synthesis, the VFA stoichiometric model could be reexpressed as \[CH₄=0.8(0.5Ace-0.25Pro+0.5But-0.25Val)\] (model 2). The root mean square prediction error (rMSPE=0.18) for model 2 was less than for model 1 (rMSPE =0.60). In addition, the bias, slope and random error of the model 2 were 2.1%, 5.7%, 92.3%, respectively, indicating that fixed error was less than 10%. In model 1, hydrogen formation resulting from VFA production were assumed to be totally consumed by methanogens for CH₄ synthesis, without considering other pathways of hydrogen metabolism, which was the main factor resulting in the higher predicted values than the measured values.