The “Novel Assessment of Nutrition and Ageing” (NANA) toolkit is a computerized system for collecting longitudinal information about older adults’ health and behavior. Here, we describe the validation of six items for measuring older adults’ self-reported mood and appetite as part of the NANA system. In Study 1, 48 community-living older adults (aged 65-89 years) completed NANA measures of their current mood and appetite alongside standard paper measures, on three occasions, in a laboratory setting. In Study 2, 40 community-living older adults (aged 64-88 years) completed daily NANA measures of momentary mood and appetite in their own homes, unsupervised, alongside additional measures of health and behavior, over three 7-day periods. The NANA measures were significantly correlated with standard measures of mood and appetite, and showed stability over time. They show utility for tracking mood and appetite longitudinally, and for better understanding links with other aspects of health and behavior.