The country’s highest court ruled that the government had failed to provide a legal basis for such a deployment, which is only permitted by law in exceptional circumstances.
The Supreme Court, with a conservative majority, therefore maintained a blockage which had been decided before it by the federal courts.
The executive had justified the use of the National Guard, a reserve unit, to protect federal agents implementing the policy of expulsions of illegal immigrants.
The move is a setback for the US president, although its significance beyond Chicago is not immediately clear.
Donald Trump ordered the deployment of National Guards in Los Angeles, Washington and Memphis to fight crime and support immigration enforcement.
These deployments have been challenged in court by his opponents, who accuse him of trampling on the limits of presidential power.
The courts blocked a similar deployment in Portland (West Oregon) in October until further notice.
