Context Total ruminal volatile fatty acids (VFA) or acetate concentrations were previously found to be moderate correlated proxies to select sheep that are genetically low methane (CH4) emitters. However, this was based on trials, with sheep fed lucerne pellets at a fixed feeding level, which is different from pastoral farming conditions in New Zealand, where the correlated proxy would be applied. Aim To determine repeatability and individual-level correlation of rumen VFAs with CH4 emissions in sheep fed ad libitum cut pasture in three and four repeated periods in Experiments 1 and 2 respectively. Sheep in Experiment 1 were also fed lucerne pellets at 2.0 × maintenance-energy requirements in two periods. Methods Methane emissions were measured from 96 and 72 animals, in Experiments 1 and 2 respectively, in respiration chambers and rumen samples were collected via oral stomach tubing before morning feeding. Repeatability estimates between periods within feed and experiment serve as an upper threshold for the estimate of heritability and ri estimates are a proxy for genetic correlation. Key results Methane (g/day) production and yield (g/kg dry-matter intake) were low to moderately repeatable traits on pasture across periods (0.58 and 0.39 for CH4 production and 0.43 and 0.32 for yield in Experiments 1 and 2 respectively). On pasture, repeatability was generally greater for VFA proportions (0.13–0.32) than for VFA concentrations (0.02–0.24), while the opposite was the case on lucerne pellets. Rumen propionate as a proportion of total VFA had strong negative ri (−0.82 and −0.87) and acetate:propionate ratio (A:P; 0.82 and 0.78) and (acetate + butyrate):(propionate + valerate) ratio (AB:PV; 0.84 and 0.82) had a strong positive ri with CH4 yield in sheep fed cut pasture, while the ri of total ruminal VFA (−0.13 and 0.35) and acetate (−0.08 and 0.38) concentrations with CH4 yield were only moderate and non-significant. Conclusion The VFA traits propionate proportion and A:P and AB:PV ratios had strong individual-level correlations with CH4 yield in sheep fed pasture ad libitum, suggesting that they would be useful correlated proxies to rank sheep CH4 yields.