In ansible, how do I specify an exclusion set of hosts in a playbook?

You specify the hosts for a playbook on the line that begins with hosts:.

From the documentation:

The hosts line is a list of one or more groups or host patterns, separated by colons, as described in the Working with Patterns documentation.

For example:

---
- hosts: all,!ntpservers
  tasks:
    # ... your tasks here
  roles:
    # ... etc etc etc

These roles and tasks will be appled to all hosts except ntpservers.