No. Use of deployed resources isn't Pulumi's domain; only creation / destruction / configuration.
Random deployment of deliberately-misconfigured network resources would overlap with this, but it wouldn't be a complete solution. Chaos monkey works in large part through stressing certain connections (high DB loads, chewing up most or all of the CPU on your load balancer, etc.), and Pulumi can't help with any of that.
You could write a chaos app that leverages Pulumi to do some of the work (and I bet the community would love to see it!).