Officers said an adult falcon and her three chicks were targeted in Houghton Quarry on 31 May.
The alert was raised after a falconer observing the nest became suspicious when the mother appeared to have stopped moving.
Pc Nick Pearson, wildlife crime officer for Northumbria Police, described the attack as "cruel and selfish".
He said: "Our initial enquiries suggest the birds have been poisoned deliberately and we are currently carrying out further enquiries to confirm which substances may have been used.
"I would appeal to anyone with information about this incident to come forward and help us identify those people whose selfish actions have deprived the region of the presence of these majestic birds."
There are about 1,500 breeding pairs of peregrine falcons in the UK.
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