Food and nutrition security is critical for economic development due to the role of nutrition in healthy growth and human capital development. Slum residents, already grossly affected by chronic poverty, are highly vulnerable to different forms of shocks, including those arising from political instability. This study describes the food security situation among slum residents in Nairobi, with specific focus on vulnerability associated with the 2007/2008 postelection crisis in Kenya. The study from which the data is drawn was nested within the Nairobi Urban Health and Demographic Surveillance System (NUHDSS), which follows about 70,000 individuals from close to 30,000 households in two slums in Nairobi, Kenya. The study triangulates data from qualitative and quantitative sources. It uses qualitative data from 10 focus group discussions with community members and 12 key-informant interviews with community opinion leaders conducted in November 2010, and quantitative data involving about 3,000 households randomly sampled from the NUHDSS database in three rounds of data collection between March 2011 and January 2012. Food security was defined using the Household Food Insecurity Access Scale (HFIAS) criteria. The study found high prevalence of food insecurity; 85% of the households were food insecure, with 50% being severely food insecure. Factors associated with food security include level of income, source of livelihood, household size, dependence ratio; illness, perceived insecurity and slum of residence. The qualitative narratives highlighted household vulnerability to food insecurity as commonplace but critical during times of crisis. Respondents indicated that residents in the slums generally eat for bare survival, with little concern for quality. The narratives described heightened vulnerability during the 2007/2008 postelection violence in Kenya in the perception of slum residents. Prices of staple foods like maize flour doubled and simultaneously household purchasing power was eroded due to worsened unemployment situation. The use of negative coping strategies to address food insecurity such as reducing the number of meals, reducing food variety and quality, scavenging, and eating street foods was prevalent. In conclusion, this study describes the deeply intertwined nature of chronic poverty and acute crisis, and the subsequent high levels of food insecurity in urban slum settings. Households are extremely vulnerable to food insecurity; the situation worsening during periods of crisis in the perception of slum residents, engendering frequent use of negative coping strategies. Effective response to addressing vulnerability to household food insecurity among the urban poor should focus on both the underlying vulnerabilities of households due to chronic poverty and added impacts of acute crises.