The Kittiwake gull was found at a roundabout in the Inshes area of Inverness on Thursday.
It was taken into care by an officer from the Scottish SPCA but had to be put to sleep.
Scottish SPCA chief inspector Iain Allan said: "The bolt had entered the gull's chest and it appears to have been targeted at close range.
"This was a sickening incident which would have caused this bird a great deal of pain and suffering.
"We can't be sure where the attack took place as it's likely the gull was still able to fly after being shot."
This is the second incident of this kind to happen this year.
In February a Herring gull was found Mile End Place in the Charleston area of Inverness with a crossbow bolt through its neck.
It also had to be put down due to its injuries.
Under the Wildlife and Countryside Act 1981 it is a criminal offence to intentionally kill or injure any wild bird using a crossbow.
The Scottish SPCA has asked anyone with information about these attacks to call their helpline on 03000 999 999.