Short Answer is: No Long Answer is: VPCs can have multiple CIDR ranges but a Subnet can only have a single IPv4 and IPv6 range assigned. As NAT devices have endpoints in the Subnet they can only be allocated a single IP per Subnet. Alternate Solution is: You could create multiple public subnets. The first set of subnets could be out of the primary CIDR and the second set of subnets with IPs out of the secondary CIDR(s). Then when creating the NAT have endpoints created in all subnets.
The question is why would you want a NAT Gateway to have 2 IPs? As both IPs would be considered "VPC Local" you would route to both IPs the same. The would be no real reason to want 2 IPs on the NAT device.
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