Background: Seamounts have been identified as aggregating locations for pelagic biodiversity including tuna; however the topography and prevailing oceanography differ between seamounts and not all are important for tuna. Although a relatively common feature in oceanic ecosystems, little information is available that identifies those that are biologically important. Improved knowledge offers opportunities for unique management of these areas, which may advance the sustainable management of oceanic resources. In this study, we evaluate the existence of an association between seamounts and tuna longline fisheries at the ocean basin scale, identify significant seamounts for tuna in the western and central Pacific Ocean, and quantify the seamount contribution to the tuna longline catch. Methodology/Principal Findings: We use data collected for the Western and Central Pacific Ocean for bigeye, yellowfin, and albacore tuna at the ocean basin scale. GLMs were applied to a coupled dataset of longline fisheries catch and effort, and seamount location information. The analyses show that seamounts may be associated with an annual longline combined catch of 35 thousand tonnes, with higher catch apparent for yellowfin, bigeye, and albacore tuna on 17%, 14%, and 14% of seamounts respectively. In contrast 14%, 18%, and 20% of seamounts had significantly lower catches for yellowfin, bigeye and albacore tuna respectively. Studying catch data in relation to seamount positions presents several challenges such as bias in location of seamounts, or lack of spatial resolution of fisheries data. Whilst we recognize these limitations the criteria used for detecting significant seamounts were conservative and the error in identification is likely to be low albeit unknown. Conclusions/Significance: Seamounts throughout the study area were found to either enhance or reduce tuna catch. This indicates that management of seamounts is important Pacific-wide, but management approaches must take account of local conditions. Management of tuna and biodiversity resources in the region would benefit from considering such effects.