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The study investigated the relationship between library instruction programme components and students' catalogue use in colleges of education libraries. The study addressed the issue of students' inability to use catalogue to retrieve materials within the libraries. Four objectives guided the study with four null hypotheses tested. Survey research deign was used for the study. The population was 2,560 NCE III students chosen from four colleges of education in south-western Nigeria. While 256 samples were used for the study, Questionnaire was used for data collection. Data gathered was analyzed using Pearson Product Moment Correlation (PPMC) coefficient for hypotheses tested. The study revealed among others that there was significant relationship between library instruction teaching methods and students library catalogue use. One of the recommendations made is that teaching methods should be improved through individual or groups assignment and computer assisted instruction should be combined with demonstration method. The study concluded that the low student’s library catalogue use could be hinged on the teaching methods, bibliographic elements.