Similar to vehicles on roadways, trains frequently kill wildlife via collisions along railways. Despite the prevalence of this mortality worldwide, little is known about the relative importance of wildlife attractants associated with railways, including spilled agricultural products, enhanced vegetation, invertebrates, and carcasses of rail-killed ungulates. We assessed the relative importance of several railway attractants to a provincially-threatened population of grizzly bears (Ursus arctos) in Banff and Yoho National Parks, Canada, for which rail-caused mortality has increased in recent decades without known cause. We examined the relationship between the use of the railway and diet by fitting 21 grizzly bears with GPS collars in 2011-2013 and measuring the stable isotope values (δ15N, δ34S) derived from their hair. We also examined the importance of rail-associated foods to grizzly bears by analyzing 230 grizzly bear scats collected from May through October in 2012-2014, some of which could be attributed to GPS-collared bears. Among the 21 collared bears, 17 used the rail rarely (<9% of the days they were monitored), and only four bears (which included the three smallest bears and the largest bear in our sample) used the rail frequently (>20% of their monitored days). We found no significant relationships between δ15N and δ34S values measured from the hair of grizzlies and their frequency of rail use. Instead, δ15N increased with body mass, especially for male bears, suggesting large males consumed more animal protein during hair growth. All four bears that used the railway frequently produced scats containing grain. Almost half the scats (43%) collected within 150 m of the railway contained grain compared to only 7% of scats found >150 m from the railway. Scats deposited near the rail were also more likely to contain grain in the fall (85% of scats) compared to summer (14%) and spring (17%), and those containing grain were more diverse in their contents (6.8 ± 2.2 species vs. 4.9 ± 1.6, P < 0.001). Lastly, scats collected near the rail were more likely to contain ungulate hair and ant remains, especially in the summer. Our results support local management knowledge that some bears in the region use the railway to forage and supplement their diets with spilled grain, but that individual use of the railway and associated foods were highly variable. We suggest that managers continue to reduce the risk of bears being killed by trains by reactively removing grain and ungulate carcasses from the railway, reducing the amount of grain spilled by trains, and target mitigation to the specific individuals and locations that attract recurrent rail-based foraging.