Criminality is currently threatening human existence on earth. Criminals are becoming more sophisticated, and have increasingly become more and more difficult to apprehend. Criminality in Nigeria has caused monumental loss of lives and properties including death of several law enforcement agents. It has also been blamed for low foreign direct investment. Huge resources have been expended on fighting crime, without much success, it makes sense then to apply psychological measures, especially to apprehending and identifying criminal. This study on Personality and Psychological Health, compared a total number of 158 participants (comprising crime suspects and non-suspects ‘Part-time students’), who were purposively and randomly selected from Nigeria Prisons, Awka division and NnamdiAzikiwe University, Awka. Their ages ranged between 20 and 35years, with the mean age of 28.23 and standard deviation of 4.40. The inclusion criteria for prison inmates (crime suspects) was having been arrested and detained in prison for a minimum period of one week and having attempted senior school certificate, while that of the undergraduates was based on their age. The Social Cognitive Theory by Bandura (1977), which claims that behaviour, is explained as guided by cognitions between the stimulus and response seems to provide possible explanation on the relationship between personality, psychological health and crime. The Big Five Personality Inventory (BFI) by John, Donahue, and Kentle (1991) and the 12-Item General Health Questionnaire (GHQ-12) by Goldberg and Williams, (1988) were used for data collection. The result of Zero-Order Correlation Matrix Coefficients showed that: “Personality traits correlated with domains of psychological health among crime suspects and non-suspects in Anambra State; while that of Multiple Analysis of Variance showed that (i) crime suspects differed significantly only in the trait of extraversion and (ii) crime suspects differed significantly from non-suspects in the domains of psychological health. Based on the findings, it was recommended amongst others that besides being useful in the pursuit for apprehending/identifying possible perpetrators of crime, Judicial Panels and the Courts should note the health status of individuals before adjudication, during incarceration, and at the point of discharge from prison. This will enable authorities concerned to treat the people affected before letting them back into the society.