TL;DR:
This script deploys the content of your deployment package on the virtual machine that you're preparing. In the case of an Angular ASP.NET Core app, this means that you will have to install IIS, the .NET Core Windows Server Hosting Bundle and copy your app to IIS.
Extra info
The Azure Virtual Machine Scale Set Deployment template creates an environment with two tasks:
- Build immutable machine image
- Azure VMSS: update with immutable machine image
Both tasks have a bunch of fields that need to be configured. Release Management allows you to link important fields to your process. This means that these settings are all grouped under the environment and can be easily set without going through the tasks.
If you look at the following screenshot you'll see that beneath the selected Deployment script field there is a line: This field is linked to 1 setting in 'Build immutable machine image'.

If you look at the documentation for the Build immutable machine image tasks you see the following for the Deployment script:
- Deployment Script: Specify the relative path to the PowerShell script (for Windows) or shell script (for Linux) that deploys the package. This script should be within the deployment package path selected above. For example, Deploy/ubuntu/deployNodejsApp.sh. The script may need to install Curl, Node.js, NGINX, and PM2; copy the application; and then configure NGINX and PM2 to run the application.
So this is the script that will automatically deploy your application to a VM. In the case of an Angular ASP.NET Core app, this means that you will have to install IIS, install the NET Core Windows Server Hosting bundle and copy your app to IIS.
I would encourage you to first create an empty Windows Server 2016 VM and experiment with creating a script that prepares the VM and installs your app. Once that's done, you can reuse this script in the Build Image task in VSTS to automate VM and image creation and use that image for your Scale Set.
UPDATE
Your VSTS Build produces an artifact. In your scenario, you are already publishing the zip file with your web application. You can configure the Publish Build Artifacts task to also publish any deployment scripts you want to use during your release. These scripts should be stored in version control. The whole artifact, including your zip file and any deployment scripts you add, is used as input to your Release Definition. The zip file contains your web app as a Web Deploy package that you need to deploy to IIS. This piece of documentation explains how to install Web Deploy and use it to deploy your app.