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Self-regulation is a complex, multifaceted concept that can be described as a higher mental process oriented toward children’s (and adults’) metacognitive, motivational, and behaviorally active participation in their own learning. It includes cognitive, behavioral, social, and emotional development. It is related to several other higher mental processes, notably executive function, and the two are sometimes confused and even conflated. They are, however, not interchangeable, and it is vital to clarify both what self-regulation is and what it is not. Failure to do so may lead to confusion at practice and policy levels, and ineffective or inappropriate practice, potentially disadvantageous to young children. Self-regulation may be significant in all aspects of development, particularly in early childhood, and efforts to enhance children’s self-regulation may be among the most effective educational interventions. Interest is reflected in developments in the field of assessment, including by the Organisation for Economic Co-operation and Development, and in government policy in, inter alia, England. Play, particularly pretense, problem-solving, and talk (both private speech and dialogue) are advocated as rich, naturalistic contexts for the development, support, and meaningful assessment of young children’s self-regulation. Some specific approaches to assessment are identified, notably observation and stimulated recall, in the form of reflective dialogues, including the use of video. Decontextualized assessment is suggested as a potentially less effective approach in capturing the full depth and range of young children’s self-regulatory competence.