the structure most responsible for maintaining cell homeostasis is the...
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the boundary between the external environment and the interior of the cell, the cell's membrane.
its not the cell membrane because it just helps in osmoregulation. but nucleus is responsible for overall homeostasis.
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The cell membrane is responsible for much more than regulation of dissolved solutes as you suggest, and although i agree the nucleus plays a large part in it, the proteome plays a larger and more direct role in "maintaing regulated internal conditions" than the nucleus. However, I would argue that the membrane, decorated with glycoproteins, is most responsible for "sensing" the environment and, yes, further relaying signals to other organelles. Without the detection, interpretation of the signals, and initiation of signalling cascades, the nucleus would not know what to transcribe in an event of an environmental change.