Students' careers are important in their lives because they will have to make decisions about their careers later in life. This study aims to examine the key predictors of Career Maturity between Vocational Aspiration and Self-Concept among the senior secondary school adolescents. Three measures are employed in the quantitative study design, including a self-concept questionnaire developed and normed by Saraswat (2011), the Occupational Aspiration Scale by J.S. Grewal (2011), and the Career Maturity Inventory by Nirmala Gupta (2013). These scales disseminated to students from the four senior secondary government and private schools of Kannauj district. Using the simple random sampling method, a total of 376 senior secondary school adolescents were involved in the study. The findings show that among senior secondary school students enrolled in both government and private institutions, vocational aspiration became a significant factor in predicting career maturity. Career Maturity was found to have significant correlation with Vocational Aspiration while no relationship was found with self-concept for total sample and sub samples. Female students were found to have better Career Maturity than males while opposite trend was seen for Vocational Aspiration. Although, the self-concept of males and females was observed to be similar. Moreover, Female students have better capability to make or choose proper vocational choices, including awareness required for choosing career according to their skills, interests, values and personality traits. However, male students were having more aspirations for the career or vocation.